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Ephemera collected by Geo. Gregory Smart related to the memory and popular image of George Washington. The collection includes postcards, calendars, cigar boxes covers, stamps and first day covers, programs for anniversary events, books and pamphlets, hat stands, billheads, stationary, cartes-de-visite, playing cards, and puzzles. Some items are catchy such as a hat stand touting the motto "friends you can hang your hat on," while others are designed to be more educational such as grade-school primers or the story of the presidents from the makers of Planters peanuts.

The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Some of the earliest photographs of the estate were created and sold to visitors by the Association as a means of income. Those efforts helped to establish an important collection of 19th century views. The collection spans the 1850s to 2000s and includes over 140 linear feet of analog material providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, and changes throughout the estate.

This collection consists of papers collected by various members of the Peter families. It includes letters from George Washington, letters of condolence to Martha Washington after George Washington's death, estate documents, Major George Peter's military papers, land plats and surveys, photo albums, letterbooks, and notebooks that tell of the life of this prominent family in Virginia and the City of Washington.

The Historical Photograph Collection is largely comprised of materials created by or for the Mount Vernon Ladies' Association. Photographers primarily include staff members and contract photographers. The collection spans the 1930s to the 2000s and includes analog material made up of a variety of sizes of film negatives providing a visual history of the Mansion, outbuildings, tombs, grounds, events, visitors, collection objects, personnel, restoration, and changes throughout the estate.

Views of Mount Vernon spanning more than 100 years. The Robert Waldsmith Collection consists of approximately 300 stereographs and cabinet cards by Alexander Gardner, N. G. Johnson, Luke D. Dillon, and others. Highlights of the collection include: several west front views of the Mansion, including the earlist known one by Frederick Langenheim, circa 1856; an early view of the tomb, circa 1857, and a collection of Washington statues and buildings honoring the first President.

The collection includes 185 titles spanning 200 years; all related to George Washington, his family, and Mount Vernon.

This collection contains correspondence, legal documents, financial records, and other documents related to John Augustine Washington III and his family, especially his son, Lawrence, as well as his granddaughters, Anne and Patty. The bulk of the correspondence series are letters sent to John Augustine Washington III and concern family affairs and the management of various family plantations, including Mount Vernon.